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Rationalized Volcano Plot in Heterogeneous Electrochemiluminescence.

Alessandro Fracassa1, Michele Orza1,2, Chiara Mariani1

  • 1Department of Chemistry "Giacomo Ciamician", Alma Mater Studiorum - University of Bologna, Bologna 40129, Italy.

ACS Electrochemistry
|May 13, 2026
PubMed
Summary
This summary is machine-generated.

Optimizing electrochemiluminescence (ECL) assays requires understanding radical stability. This study reveals a volcano-type relationship between radical cation deprotonation rates and ECL intensity, defining an optimal stability window for enhanced emission.

Keywords:
DFTECL emitting layerbead-based assaykineticsradical deprotonation

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Area of Science:

  • Analytical Chemistry
  • Electrochemistry
  • Spectroscopy

Background:

  • Electrocatalysis performance relies on electrogenerated coreactant radical stability.
  • Radical stability dictates the spatial extent of the electrochemiluminescence (ECL) emitting layer.
  • Existing methods struggle to correlate ECL intensity with intrinsic radical stability.

Purpose of the Study:

  • To establish a direct correlation between ECL intensity and intrinsic deprotonation kinetics of radical cations.
  • To investigate the impact of radical cation stability on ECL emission efficiency.
  • To identify an optimal stability window for efficient ECL assays.

Main Methods:

  • Utilized ECL microscopy to correlate individual [Ru-(bpy)3]2+-labeled bead intensity with radical cation deprotonation kinetics.
  • Employed density functional theory (DFT) calculations with a hybrid cluster-continuum approach.
  • Investigated model electrogenerated radical cations, including a novel aniline derivative.

Main Results:

  • Disentangled intrinsic radical decomposition rates from experimental artifacts (pH, buffer effects).
  • Revealed a non-monotonic, volcano-type dependence between deprotonation rate and ECL intensity.
  • Identified an optimal stability window for radical cations, crucial for efficient ECL emission.

Conclusions:

  • Radical cation stability is a critical parameter for optimizing ECL assay performance.
  • The identified volcano-type relationship provides a new framework for designing stable radical intermediates.
  • This work paves the way for rational design of improved ECL assays with enhanced sensitivity and efficiency.